Matthew Lohr

Suppression of the coffee-ring effect by shape-dependent capillary interactions

When a drop of liquid dries on a solid surface, its suspended particulate matter is deposited in ring-like fashion. This phenomenon, known as the coffee-ring effect, is familiar to anyone who has observed a drop of coffee dry. During the drying process, drop edges become pinned to the substrate, and capillary flow outward from the centre of the drop brings suspended particles to the edge as evaporation proceeds. After evaporation, suspended particles are left highly concentrated along the original drop edge. The coffee-ring effect is manifested in systems with diverse constituents, ranging from large colloids to nanoparticles and individual molecules. In fact—despite the many practical applications for uniform coatings in printing, biology and complex assembly—the ubiquitous nature of the effect has made it difficult to avoid. Here we show experimentally that the shape of the suspended particles is important and can be used to eliminate the coffee-ring effect: ellipsoidal particles are deposited uniformly during evaporation. The anisotropic shape of the particles significantly deforms interfaces, producing strong interparticle capillary interactions. Thus, after the ellipsoids are carried to the air–water interface by the same outward flow that causes the coffee-ring effect for spheres, strong long-ranged interparticle attractions between ellipsoids lead to the formation of loosely packed or arrested structures on the air–water interface. These structures prevent the suspended particles from reaching the drop edge and ensure uniform deposition. Interestingly, under appropriate conditions, suspensions of spheres mixed with a small number of ellipsoids also produce uniform deposition. Thus, particle shape provides a convenient parameter to control the deposition of particles, without modification of particle or solvent chemistry.

Effects of particle shape on growth dynamics at edges of evaporating drops of colloidal suspensions.

We study the influence of particle shape on growth processes at the edges of evaporating drops. Aqueous suspensions of colloidal particles evaporate on glass slides, and convective flows during evaporation carry particles from drop center to drop edge, where they accumulate. The resulting particle deposits grow inhomogeneously from the edge in two dimensions, and the deposition front, or growth line, varies spatiotemporally. Measurements of the fluctuations of the deposition front during evaporation enable us to identify distinct growth processes that depend strongly on particle shape. Sphere deposition exhibits a classic Poisson-like growth process; deposition of slightly anisotropic particles, however, belongs to the Kardar-Parisi-Zhang universality class, and deposition of highly anisotropic ellipsoids appears to belong to a third universality class, characterized by Kardar-Parisi-Zhang fluctuations in the presence of quenched disorder.

Helical Packings and Phase Transformations of Soft Spheres in Cylinders

The phase behavior of helical packings of thermoresponsive microspheres inside glass capillaries is studied as a function of the volume fraction. Stable packings with long-range orientational order appear to evolve abruptly to disordered states as the particle volume fraction is reduced, consistent with recent hard-sphere simulations. We quantify this transition using correlations and susceptibilities of the orientational order parameter psi6. The emergence of coexisting metastable packings, as well as coexisting ordered and disordered states, is also observed. These findings support the notion of phase-transition-like behavior in quasi-one-dimensional systems.